Articles

https://doi.org/10.1038/s41928-021-00671-0

Mobility–stability trade-off in oxide thin-film

transistors
Yu-Shien Shiah1, Kihyung Sim1, Yuhao Shi1, Katsumi Abe2, Shigenori Ueda 3
, Masato Sasase1,
Junghwan Kim 1 ✉ and Hideo Hosono 1,3 ✉

Thin-film transistors based on amorphous oxide semiconductors could be used to create low-cost backplane technology for
large flat-panel displays. However, a trade-off between mobility and stability has limited the ability of such devices to replace
current polycrystalline silicon technologies. Here we show that the sensitivity of amorphous oxide semiconductors to externally
introduced impurities and defects is determined by the location of the conduction-band minimum and the relevant doping abil-
ity. Using bilayer-structured thin-film transistors, we identify the exact charge-trapping position under bias stress, which shows
that the Fermi-level shift in the active layer can occur via electron donation from carbon-monoxide-related impurities. This
mechanism is highly dependent on the location of the conduction-band minimum and explains why carbon-monoxide-related
impurities greatly affect the stability of high-mobility indium tin zinc oxide transistors but not that of low-mobility indium gal-
lium zinc oxide transistors. Based on these insights, we develop indium tin zinc oxide transistors with mobilities of 70 cm2 (V s)–1
and low threshold voltage shifts of –0.02 V and 0.12 V under negative- and positive-bias temperature stress, respectively.

A
morphous oxide semiconductors (AOSs), such as indium
gallium zinc oxide (IGZO), are promising channel mate-
rials for thin-film transistors (TFTs) used in flat-panel
displays due to their high mobility, good uniformity over large
areas, low-temperature processability and optical transparency1.
AOS-based pixel-driven devices have already been commercialized
for use in small state-of-the-art displays. However, the next genera-
tion of display technologies require TFTs with an electron mobility
greater than 10 cm2 (V s)–1 that can be substantially higher in some
cases. For example, super-high-vision technology, which mostly
uses organic light-emitting diodes (LEDs) or quantum-dot LEDs,
requires TFTs with an electron mobility higher than 40 cm2 (V s)–1
(ref. 2). High-mobility AOSs can also be used in non-display fields,
including chip input/output, image sensors and power systems3–5.
Furthermore, for power systems, the intrinsic properties of AOSs
such as their wide bandgap, low-temperature process and high
mobility can help with high-voltage operation and reduce power
dissipation with compatible on-chip processes.
A range of high-mobility AOSs have already been explored.
However, serious stability problems under bias testing have been
observed in high-mobility AOSs. Negative-bias temperature stress
(NBTS), positive-bias temperature stress (PBTS) and negative-bias
illumination stress (NBIS) are the core tests used to evaluate the
reliability of TFTs. NBTS stability tends to degrade with an increase
in the field-effect mobility and this instability is highly dependent
on the chemical composition of the AOS. Electron mobility signifi-
cantly differs depending on conduction-band dispersion, which is
mainly governed by the magnitude of spatial overlap between the
post-transition metal cations6. For example, low-mobility indium
gallium oxide (InGaOx; IGO) TFTs exhibit high NBTS stability,
whereas high-mobility indium tin zinc oxide (InSnZnOx; ITZO)
TFTs exhibit low NBTS stability. This mobility–stability trade-off is
well known, but no scientific reasoning has been reported to explain
the correlation (NBTS stabilities are compared in Supplementary
Table 1 and Supplementary Fig. 1a,b).
In this Article, we report a solution to the mobility–stability
trade-off observed in AOS TFTs. We focus on the NBTS mecha-
nism, the correlation of electronic structures with NBTS and
the possible origins of NBTS. We show that (1) NBTS is due to a
Fermi-level shift (change in carrier density) of the AOS itself, (2) the
deep conduction-band minimum (CBM) of high-mobility AOSs
prefers to accept electrons from the outside and (3) carbon monox-
ide (CO)-related impurities donate electrons to the CBM of AOSs at
room-temperature NBTS (also referred to as NBS here). Based on
this understanding, we develop ultrastable ITZO TFTs with mobili-
ties of 70 cm2 (V s−1).
Identification of NBTS mechanism utilizing bilayer
channels
Conventionally, charge trapping in the gate insulator is used as a
model to explain the shift in the threshold voltage (Vth) in tran-
sistors. As illustrated in Fig. 1a, positive charges trapped at the
gate-insulator interface induce electron accumulation near the gate
insulator at gate voltage VG = 0 V. There are several candidates for
the positive charges, such as holes (h+), protons (H+) and ionized
oxygen vacancies (VO+). In fact, there have been some reports on
NBTS in AOS TFTs based on this model7. However, we were doubt-
ful whether charge trapping at the gate insulator can explain the dif-
ferences in behaviours between high- and low-mobility AOSs. To
validate the charge-trapping model, the following criteria should
be satisfied: high-mobility AOSs must possess a higher hole density
or mobility; high-mobility AOSs must possess higher hydrogens or
proton conductivity; and high-mobility AOSs must possess a much
smaller hole-injection barrier against the gate insulator. However,
we determined that these criteria are impractical. For example, IGO
and ITZO possess similar ionization potentials of ~7.2 eV, implying
that both have a similar hole-injection barrier height against the gate
insulator. Moreover, it was confirmed that the number of hydro-
gens incorporated in IGO and ITZO are fairly similar. Therefore,
we excluded the charge-trapping model in the gate insulator and

1
Materials Research Center for Element Strategy, Tokyo Institute of Technology, Yokohama, Japan. 2Silvaco, Kyoto, Japan. 3WPI-MANA, National Institute
for Materials Science, Ibaraki, Japan. ✉e-mail: JH.KIM@mces.titech.ac.jp; hosono@mces.titech.ac.jp

800 Nature Electronics | VOL 4 | November 2021 | 800–807 | www.nature.com/natureelectronics

Nature Electronics
a b
CBM CBM
EF
EF (after bias)
Drain current (A)
Gate insulator
Gate insulator
EF (initial)
VBM VBM
Fig. 1 | Schematic of two possible NBS mechanisms. a, Gate-insulator charge-trapping model. b, AOS Fermi-level shift model. c, Transfer curves of
amorphous ITZO thin-film transistor with various carrier densities obtained by simulation. (CBM, VBM and EF denote conduction band maximum, valence
band maximum and Fermi level energy, respectively).
focused on the possibility of the Fermi-level shift or change in car-
rier density of the AOS itself, as illustrated in Fig. 1b.
It is well known that the carrier density is closely related to Vth
in TFTs. To determine how Vth differs for different carrier densi-
ties, we performed device simulation. Figure 1c presents the simula-
tion results, which reveal that the Vth shift (ΔVth) became significant
when the carrier density was >1017 cm−3: ΔVth was –6.0 V when the
carrier density increased from 1 × 1017 to 5 × 1017 cm−3 and it was
–13.5 V when the carrier density increased from 1017 to 1018 cm−3.
This result implies that the NBTS phenomenon may occur if the
carrier density in bulk AOS increases during the bias stress test.
However, it is almost impossible to determine which model should
be applied to the observed NBTS because the final transfer curves
are the same irrespective of the mechanisms displayed in Fig. 1a,b.
Therefore, identifying the dominant NBTS mechanism is critical to
determine the origin of the trade-off.
Here we propose a method to easily identify the NBTS
mechanism. As illustrated in Fig. 2a, a bottom-gate TFT with a
bilayer active-channel structure was employed. One layer was
an NBTS-stable AOS, whereas the other was an NBTS-unstable
AOS. We employed IGO and ITZO for this purpose, and their
single-layer TFT characteristics are presented in Fig. 2b,c, respec-
tively. The stacking order should be noted: the NBTS-stable layer
(IGO) is adjacent to the gate insulator, and the NBTS-unstable layer
(ITZO) is outermost from the gate insulator. This bilayer struc-
ture enables to distinguish the two NBTS mechanisms by observ-
ing the relationship between the field-effect mobility and VG. As
displayed in Supplementary Fig. 2a, a key point is that IGO and
ITZO exhibit fairly different tendencies in the field-effect mobil-
ity versus VG curve, owing to the very different electron mobilities
(IGO: ~20 cm2 (V s)–1; ITZO: ~50 cm2 (V s)–1). Namely, we can iden-
tify which channel is open and which channel’s Vth varies from the
field-effect mobility versus VG curve.
Figure 2d,e presents the device simulation results corresponding to
the gate-insulator charge-trapping model and Fermi-level shift model,
respectively. It is worth noting that the two different NBTS mecha-
nisms result in obviously different tendencies. The gate-insulator
charge-trapping model results in a parallel shift in the field-effect
mobility versus VG curve, as shown in Fig. 2d. For the Fermi-level
shift model, we should focus on the region of negative-differential
field-effect mobility. This region is attributed to the mode shift from
the bilayer channel (ITZO/IGO) to single-layer channel (IGO layer).
Nature Electronics | VOL 4 | November 2021 | 800–807 | www.nature.com/natureelectronics
Articles
c
10–4
10–6
10–8
Carrier density
(×1017 cm–3)
–10
10
0.1
10 –12 0.5
1.0
10–14
3.0
5.0
10–16
10.0
10–18
–30 –20 –10 0 10 20 30
Gate voltage (V)
Thus, the position of the negative-differential field-effect mobil-
ity region will not change when Vth of the IGO layer is the same.
Consequently, it was confirmed that the experimental data agree well
with the Fermi-level shift (change in carrier density) model, as illus-
trated in Fig. 2e,f. This characteristic can be demonstrated by the close
agreement between the observed data and superimposed plots of the
single-layer IGO-based and ITZO-based device (Supplementary
Fig. 2b). We believe that this bilayer TFT structure can even be
extended to the identification of the PBTS or NBIS mechanism.
Electronic structure and carrier-doping ability of AOSs
Based on Fig. 2, NBTS instability was attributed to the change in the
electron density of the AOS (ITZO). The next question is to deter-
mine the dominant factor controlling the mobility of AOSs. There
exists a universal tendency in electronic structures and chemical
composition. For AOSs, the CBM mainly consists of vacant s orbit-
als of metal cations. Therefore, conduction-band dispersion is highly
dependent on the level of spatial overlap of the s orbitals of metal cat-
ions; cations with larger vacant s orbitals are more effective in achiev-
ing larger dispersion (small effective mass), as indicated in Fig. 3b,c.
Generally, ECBM tends to deepen with an increase in conduction-band
dispersion, as demonstrated in Fig. 3a. This phenomenon explains
why high-mobility AOSs consist of heavier-metal cations, such as
In and Sn. Furthermore, the variation in ECBM, namely, the electron
affinity, results in large differences in electrical properties, such
as the carrier-doping ability8. Most AOSs have a wide bandgap of
>2.5 eV; thus, the contribution of thermally excited electrons (from
the valence band) is negligible at ambient temperature, implying that
only ionized donors contribute to the carrier density.
To date, several studies have proposed possible candidates for
n-type dopants in AOSs, such as oxygen vacancy (VO) and hydro-
gens (OH− or H−)9,10. However, there have been a limited number
of studies on the carrier-doping limit in AOSs. Here we would like
to emphasize that the activation energy (Ea) of n-type dopants in
AOSs differs depending on the chemical composition.
( Ea ) In general,
the carrier density is expressed as ne = ND exp − kT , where ne, ND,
Ea, K and T denote carrier density, donor density, activation energy,
Boltzmann constant and temperature, respectively. The carrier den-
sity significantly varies according to Ea, as indicated in Fig. 3d, even
if the donor densities are the same. Evidently, ND should increase
from ~6 × 1016 to 3 × 1018 cm−3 when Ea changes from 0.05 to 0.15 eV
to obtain ne = 1016 cm−3. Namely, the required donor densities
801
Articles Nature Electronics

a b 10–4 c 10–4
IGO single-layer TFT ITZO single-layer TFT
Source Drain W = 300 µm; L = 50 µm
10–6 10–6
VD = 0.1 V

Drain current (A)

Drain current (A)
NBTS-unstable AOS
(ITZO, 20 nm)
10–8 10–8
NBS NBS
NBTS-stable AOS
0s 0s
(IGO, 15 nm)
10–10 500 s 10–10 500 s
Interface 1,800 s 1,800 s
(IF) 3,600 s 3,600 s
SiO2 (150 nm)
10–12 10–12
Gate (p++-Si) –30 –20 –10 0 10 20 30 –30 –20 –10 0 10 20 30
Gate voltage (V) Gate voltage (V)

Device simulation

d e f
GI charge-trapping model Fermi-level shift model Experimental result
30 30 30
Interface charge at IF Carrier concentration of ITZO IGO/ITZO bilayer TFT
Field-effect mobility (cm2 (V s)–1)

Field-effect mobility (cm2 (V s)–1)

Field-effect mobility (cm2 (V s)–1)

20 20 20

NBS
10 10 10 0s
1 4 0.5 2.0
500 s
8 12 4.0 6.0
1,800 s
Positive charge (×1011 cm–2) Charge density (×1017 cm–3) 3,600 s
0 0 0
–10 0 10 20 30 –10 0 10 20 30 –30 –20 –10 0 10 20 30
Gate voltage (V) Gate voltage (V) Gate voltage (V)

Fig. 2 | Identification of NBTS mechanism utilizing bilayer TFT. a, Schematic of the device structure. b,c, Transfer curves of TFTs with single amorphous
IGO layer (b) and single amorphous ITZO layer (c) after NBS. d,e, Simulation results of field-effect mobility and gate voltage for the bilayer TFT based on
the gate-insulator (GI) charge-trapping model (d) and Fermi-level shift model (e). For the gate-insulator charge-trapping model, the positive charge at the
gate-insulator interface varied from 1.0 × 1011 to 1.2 × 1012 cm−2. For the Fermi-level shift model, the carrier density of the ITZO layer varied from 5 × 1016 to
6 × 1017 cm−3. f, Experimentally obtained data for field-effect mobility and gate voltage. For the NBS test, a negative bias of Vth −20 V was applied. Transfer
curves were taken with a drain–source voltage of 0.1 V.

become approximately 100 times different with a difference in Ea of of ND is required for AOSs with shallower donor levels and a smaller
0.1 eV. As indicated in Fig. 3e, the Ea values depend on the chemical value of ND may make ITZO to become more sensitive to defects
composition. In general, AOSs with a deep ECBM exhibit a small Ea. and impurities. In this context, we show that a large number of
However, it has been observed that Ea is also related to the ioniza- CO-related impurities were introduced after the photolithography
tion potential11,12. The origin of Ea is not discussed in this paper. The process. The thermal desorption spectra shown in Fig. 4a,b indicate
most important fact is that Ea significantly varies with the chemi- that carbon-related impurities, namely, CO and CO2, were detected
cal composition, and the necessary donor densities are different. only for the ITZO thin film that underwent the photolithography
Consequently, the difference in Ea determines the defect tolerance process, which was also confirmed by hard X-ray photoemission
of AOSs to VO and H-related defects. In other words, ne in an AOS spectroscopy (HAXPES) (Fig. 4c–f)13. The C1s peak clearly shows
with a smaller Ea is more easily affected by VO and H-related defects. the existence of C–O and C=O components; thus, the O1s peak
Here let us suppose that there are two AOSs with different ini- should also be deconvoluted at least into three components: lattice
tial values of ND: one AOS has an ND value of 1016 cm−3, whereas oxygen, C–O and C=O (refs. 14–20). It should be noted that the O1s
the other has an ND value of 1019 cm−3. In addition, VO or H-related peak at around 532 eV has been well used for the determination of
defects of 1018 cm−3 are formed in post-processing, such as photo- VO defects in this field21–23. This background implies that if we have
lithography, gate insulator and passivation process. It is expected not revealed the CO-related impurity, this study could have been
that the ND value of the AOS with initial ND of 1016 cm−3 changes to concluded as the VO-related issue because the carbon-related O1s
1018 cm−3. Thus, the defect tolerance can be defined as the degree of peak also takes the position of ~532 eV (refs. 14–20).
insensitivity to foreign impurity donors. This phenomenon explains The amounts of both CO and CO2 were revealed to be
why high-mobility AOSs, such as ITZO, are sensitive to the process- ~5 × 1015 cm−2, and Auger electron spectroscopy measurement
ing environment as well as impurities. It should be noted that the indicated that CO-related impurities existed in the surface region
high-mobility AOS itself is not a defective material. (Supplementary Fig. 3). In addition, the thermal desorption spectra
indicated that the CO-related impurities were not physisorbed spe-
CO-related impurity in AOSs and its influence on NBTS cies because the desorption temperature was high (~350 °C). Thus,
As discussed above, high-mobility AOSs, such as ITZO, have a deep the CO-related impurities were formed as a result of the chemi-
ECBM with shallow donor levels (small Ea of donors); a smaller value cal reaction between the oxide surface and alkali photoresist (PR).

802 Nature Electronics | VOL 4 | November 2021 | 800–807 | www.nature.com/natureelectronics

Nature Electronics Articles
a b c
Carrier (electron) stability 13 14 High mobility Low mobility

3s Al Si
Electron mobility
Aluminium Silicon CBM

High mobility

Deep CBM
Contribution of cation (5s) orbitals 30 31 32
CBM
2.0 4s Zn Ga Ge
Zinc Gallium Germanium
48 49 50
4.0 5s Cd In Sn VBM VBM
Energy level (eV)

Cadmium Indium Tin

Deepe ning the E CBM

6.0 d 1020
e 1018
ne = NDexp(–Ea/kT ) In0.2Sn0.4Zn0.4Ox
ne, electron density Ea = 0.06 eV
ND, donor density 1017
8.0 1018

Carrier density (cm–3)

Carrier density (cm–3)

1016

1016 In0.2Sn0.4Ga0.4Ox
10.0
1015
a-SnO2–x
a-(In0.75Zn0.25)Ox

a-(In0.50Zn0.50)Ox
a-(In0.2Sn0.4Ga0.4)Ox

a-(In0.2Sn0.4Zn0.4)Ox

a-(Sn0.75Ga0.25)Ox

a-(Sn0.50Ga0.50)Ox

a-InGaZnOx

a-(In0.25Zn0.75)Ox

a-(Ga0.35Zn0.65)Ox

a-(Ga0.70Zn0.30)Ox

a-Ga2O3–x

Ea = 0.15 eV
Ea = 0.01 eV
1014 1014
Ea = 0.05 eV
Ea = 0.10 eV
1013 Sn0.5Ga0.5Ox
Ea = 0.15 eV
1012 Ea = 0.27 eV
Ea = 0.20 eV
1012
16 17 18
10 10 10 1019 1020 3.0 3.5 4.0 4.5 5.0 5.5 6.0 6.5
Doping density (cm–3) 1,000/T (K–1)

Fig. 3 | Universal tendency of electronic structure and electrical properties of AOSs. a, CBM deepening depending on the composition of AOSs based on
post-transition metals, obtained by ultraviolet spectroscopy. b, Candidate post-transition metals for the AOS system in the periodic table. c, Schematic of
the band structures for both heavy post-transition metal oxide (high mobility) and light post-transition metal oxide (low mobility). d, Carrier concentration
as a function of donor density (ND) for a metal oxide system with different activation energies. e, Temperature dependence of carrier concentration of
representative AOSs and evaluated activation energy (Ea).

a b c
m/z = 28 m/z = 44 C1s before photolithography
Before photolithography Before photolithography
After photolithography After photolithography
QMS signal (a.u.)

QMS signal (a.u.)

Intensity (a.u.)

200 300 400 500 200 300 400 500 290 288 286 284 282
Temperature (°C) Temperature (°C) Binding energy (eV)

d e f
C1s after photolithography O1s before photolithography O1s after photolithography
Raw data
Fitting line
Intensity (a.u.)
Intensity (a.u.)

Intensity (a.u.)

Background
C–C, C–H
C–O
C=O

290 288 286 284 282 538 534 530 526 538 534 530 526
Binding energy (eV) Binding energy (eV) Binding energy (eV)

Fig. 4 | CO-related impurities introduced by photolithography. a,b, Thermal desorption spectra of mass number 28 for CO (a) and mass number
44 for CO2 (b). c–f, Surface HAXPES data of ITZO thin films: C1s peaks before (c) and after (d) photolithography; O1s peaks before (e) and after (f)
photolithography. (QMS and m/z denote quadrupole mass spectrometry and mass to charge ratio, respectively).

Nature Electronics | VOL 4 | November 2021 | 800–807 | www.nature.com/natureelectronics 803

Articles Nature Electronics

a b c
10–5 10–5
m/z = 28 No annealing after 300 °C annealing after
PR contamination 10–6 PR contamination 10–6 PR contamination
300 °C annealing
QMS signal (a.u.)

Drain current (A)

Drain current (A)

10–7 10–7
350 °C annealing
400 °C annealing 10–8 NBS 10–8
NBS
0s 0s
10–9 10–9
500 s 500 s
1,800 s 1,800 s
10–10 10–10
3,600 s 3,600 s
10–11 10–11
200 300 400 500 –30 –20 –10 0 10 20 30 –40 –30 –20 –10 0 10 20
Temperature (°C) Gate voltage (V) Gate voltage (V)

d e
10–5 10–5
350 °C annealing after 400 °C annealing after
10–6 PR contamination 10–6 PR contamination
Drain current (A)

Drain current (A)

10–7 10–7

10–8 10–8
NBS NBS
0s 0s
10–9 10–9
500 s 500 s
10–10 1,800 s 10–10 1,800 s
3,600 s 3,600 s
10–11 10–11
–30 –20 –10 0 10 20 30 –30 –20 –10 0 10 20 30
Gate voltage (V) Gate voltage (V)

Fig. 5 | Correlation between CO-related impurity and bias stability. a, Thermal desorption spectra of mass number 28 (CO) for PR-contaminated
amorphous ITZO films with different annealing temperatures. b–e, NBS results of ITZO TFT samples before annealing (b) and after annealing at 300 °C
(c), 350 °C (d) and 400 °C (e). For the NBS test, a negative bias of Vth−20 V was applied. Transfer curves were taken with a drain–source voltage of 0.1 V.

It was also confirmed that the chemical reaction is not limited to a impurities. As shown in Supplementary Fig. 8, a fairly large amount
specific PR; PRs of different companies yielded the same results, as of CO-related impurities was confirmed for the sample depos-
shown in Supplementary Fig. 4. ited in the vacuum chamber with a base pressure of ~10–5 Pa. This
Before investigating the effect of CO-related impurities on TFTs, result suggests that all the possible sources of CO-related impurities
it was first necessary to consider how to eliminate these impurities. should be considered for high-mobility AOS TFTs.
Based on the fact that all CO-related impurities desorb at >350 °C To further understand the role of CO-related impurities, we
(Fig. 4a,b), we modified the conventional TFT fabrication pro- focused on conventional CO gas sensors based on metal oxides and
cess, as illustrated in Supplementary Fig. 5: 400 °C post-annealing noticed that there have already been many studies on the charge
was performed in the final step, which made it possible to obtain transfer phenomenon between metal oxides and adsorbates by
a CO-impurity-free ITZO TFT. Next, ITZO TFTs with different Fermi-level modulation24,25. The proposed charge transfer mecha-
amounts of CO-related impurities were prepared by exposing the nism is as follows: when the Fermi level is shifted down by gate
TFTs to PR and varying the annealing temperature. Consequently, biasing, the adsorbates donate electrons to metal oxides. There
we observed a noticeable correlation between the CO amount and have also been many reports on gas sensors utilizing this mecha-
NBTS instability, as illustrated in Fig. 5. It should be noted that nism, called gas field-effect transistors24–29. Here we considered why
CO-related impurity was not limited to ITZO. Almost the same the CO-related impurities influence higher-mobility AOSs rather
number of CO-related impurities were also confirmed for conven- than the lower-mobility ones. The ECBM value is an important factor
tional AOSs after the same photolithography process, as illustrated because electrons are transferred from the adsorbates to the con-
in Supplementary Fig. 6a. Nevertheless, it is interesting to note that duction band of AOSs, implying that the deep ECBM enables to get
the IGZO TFT rarely suffers from NBTS instability even if there electrons more readily from the adsorbates. The Wolkenstein model
were the same number of CO-related impurities, as illustrated in also suggests that charge transfer from the adsorbates is strongly
Supplementary Fig. 6b. This phenomenon was most likely due to governed by the Fermi level and ECBM (ref. 29).
the mobility–stability trade-off. Only the ITZO TFT suffered from Based on conventional studies and our experimental results,
serious NBS instability by CO-related impurities. We note that the Supplementary Fig. 9a,b presents the schematic of the donor-like
NBS mechanism is based on the increase in carrier density in ITZO, states formed by CO-related impurities. It was supposed that the
implying that CO-related impurities may form donor-like states. CO-related impurities formed a deep state before gate biasing since
To clarify that the obtained NBTS stability in Fig. 5e is not attrib- there was no difference in the carrier density of ITZO samples with
utable to the thermal annealing effect, we fabricated an impurity-free and without the CO impurities. Then, a significant change in the
ITZO TFT by the shadow-mask process (width, W = 1,000 µm; carrier density appeared after NBS, indicating that the initial deep
length, L = 500 µm). As shown in Supplementary Fig. 7, the state was transformed into a shallow state. There have been a num-
shadow-mask process was revealed to greatly improve the NBTS ber of studies regarding the adsorption of CO on semiconducting
stability. This result strongly supports the correlation between the oxide surfaces30–32. The different behaviours of ITZO and IGZO
CO-related impurity and NBTS instability. On the other hand, we TFTs towards CO-related impurities may be explained based on the
also found that the residual gas can be another source of CO-related discussion above. In particular, we proposed that AOSs with large

804 Nature Electronics | VOL 4 | November 2021 | 800–807 | www.nature.com/natureelectronics

Nature Electronics Articles
a 10–5 b 10–5
c 10–5
In0.2Sn0.4Zn0.4Ox In0.2Sn0.4Zn0.4Ox In0.2Sn0.4Zn0.4Ox
–6 –6
10 50 cm2 (V s)–1 10 50 cm2 (V s)–1 10–6 50 cm2 (V s)–1
NBIS
10–7 10–7 10–7
Drain current (A)

Drain current (A)

Drain current (A)
15,000 lx

µFE (cm2 (V s)–1)

50
NBTS PBTS Dark
10–8 10–8 10–8
0s 0s 1s
30
10–9 100 s 10–9 100 s 10–9 100 s
–10 500 s –10 500 s 500 s
10 10 10 10–10
1,000 s 1,000 s 1,000 s
10–11 0 50 1,800 s 10–11 1,800 s 10–11 1,800 s
–12
VG (V) 3,600 s –12
3,600 s 3,600 s
10 10 10–12
–30 –20 –10 0 10 20 30 –30 –20 –10 0 10 20 30 –30 –20 –10 0 10 20 30
Gate voltage (V) Gate voltage (V) Gate voltage (V)
d 10–5 e 10–5 f 10–5
In0.4Sn0.4Zn0.2Ox In0.4Sn0.4Zn0.2Ox In0.4Sn0.4Zn0.2Ox
–6 –6
10 70 cm2 (V s)–1 10 70 cm2 (V s)–1 10–6 70 cm2 (V s)–1
NBIS
10–7 10–7 10–7
Drain current (A)

Drain current (A)

Drain current (A)

15,000 lx
70
µFE (cm2 (V s)–1)

10–8 NBTS 10–8 PBTS Dark

10–8
50 0s 0s 1s
–9 –9
10 100 s 10 100 s 10–9 100 s
30
–10 500 s –10 500 s 500 s
10 10 10–10
10 1,000 s 1,000 s 1,000 s
10 –11
1,800 s 10 –11 1,800 s 1,800 s
0 50 10–11
VG (V) 3,600 s 3,600 s 3,600 s
–12 –12
10 10 10–12
–30 –20 –10 0 10 20 30 –30 –20 –10 0 10 20 30 –30 –20 –10 0 10 20 30
Gate voltage (V) Gate voltage (V) Gate voltage (V)

Fig. 6 | Stability test results of ITZO TFTs with different chemical compositions. a–c, NBTS (a), PBTS (b) and NBIS (c) data for In0.2Sn0.4Zn0.4Ox TFT.
d–f, NBTS (d), PBTS (e) and NBIS (f) data for In0.4Sn0.4Zn0.2Ox TFT. For NBTS and PBTS, a positive or negative bias of Vth±20 V was applied at 60 °C.
For NBIS, illumination from a white LED light of 15,000 lx was used with a negative bias of Vth−20 V. (μFE denotes field effect mobility).

Ea, such as IGZO, are rarely affected by externally introduced impu- light-shielding layers. However, NBIS is a concern that should
rities, which can be easily understood from the formula shown in be resolved in the near future for fully transparent electronics. It
Supplementary Fig. 9c; the primary factor is the location of the ECBM. is interesting to note that NBIS is greatly improved by applying
treatment to eliminate CO-related impurities and subsequently
Ultrastable ITZO TFTs with high mobility of 70 cm2 (V s)–1 passivating ITZO with ZSO (Supplementary Fig. 11)35–37. Also,
We have shown that an NBS-stable ITZO TFT can be created by note that the IGZO TFT discussed in a previous study exhibited
eliminating CO-related impurities. However, it should be noted a large Vth shift of –9 V under the same NBIS condition38. In con-
that, in practice, TFTs are exposed to much higher stresses. In this trast, the ITZO TFTs in this study exhibited much better NBIS
respect, we conducted all the relevant stress tests: NBTS, PBTS stability (Fig. 6c,f); a small Vth shift of −0.48 V was observed for
and NBIS. To avoid surface-related problems, the ITZO active the In0.2Sn0.4Zn0.4Ox TFT. Furthermore, we attributed the relatively
layer was passivated by 5-nm-thick amorphous Zn–Si–O (ZSO) low NBIS stability of the In-rich ITZO TFT to its narrower optical
(Supplementary Figs. 10–12). The use of ZSO (ref. 33) led to the fol- bandgap (Supplementary Fig. 14).
lowing effects: (1) eliminating the surface states of ITZO and (2) Further, we compared the persistent photoconductivity of two
fully blocking charge transfer between the ITZO layer and the out- ITZO thin films (with and without a 5-nm-thick ZSO passivation
side. We also questioned what degree of mobility is practically avail- layer). As shown in Supplementary Fig. 15, the ITZO thin films were
able for AOS TFTs. Thus, we studied more In-rich ITZO, namely, illuminated for 10 min and then a time-dependent Hall measure-
In0.4Sn0.4Zn0.2Ox. ment was conducted in darkness. Surprisingly, the ITZO thin film
Consequently, we determined that the ITZO TFT with a high with ZSO exhibited almost no change in carrier density, whereas
mobility of ~70 cm2 (V s)–1 meets the requirements for practical use the carrier density of the ITZO thin film without ZSO increased
(Fig. 6 and Supplementary Table 2), which validates the potential from 2 × 1017 to 2 × 1018 cm–3, as shown in Supplementary Fig. 15a.
of ITZO TFT as an alternative to low-temperature polysilicon. In This result effectively explains why the ZSO-passivated ITZO TFT
addition, we found that PBTS is mainly caused by layers adjacent exhibits high NBIS stability. On the other hand, it should be noted
to the active layers. Simply put, when depositing the second layer, that the 5-nm-thick ZSO does not contribute to optical absorption
such as the passivation layer or gate insulator, onto the ITZO layer, owing to its wide bandgap and ultrathin thickness (Supplementary
relatively high oxygen partial pressure(PO2) is required to suppress Fig. 15b), indicating that the numbers of absorbed photons are
the reduction of the ITZO layer. Here the high PO2 may form trap almost the same for both samples. It is, thus, inferred that the pho-
states attributed to excess oxygen depending on what type of passiv- tostability of ITZO is mainly governed by surface defects such as
ation layer is used. As illustrated in Supplementary Fig. 13, serious VO. Other studies have also reported that a passivation layer of
PBTS instability occurred with 5-nm-thick amorphous Ga2Ox pas- Y2O3 effectively eliminates surface defects in IGZO (refs. 35–37).
sivation layers that were readily involved in excess oxygen-related Consequently, this study indicates that obtaining an impurity- and
trap states34. Above all, it should be noted that the use of high PO2 defect-free surface or interface is a key factor to the stability of AOS
for the second layer is also the reason why ITZO should maintain a TFTs. In this respect, d.c.-sputtering-based passivation or interlayer
small donor density (ND). (between the active layer and gate insulator) may be a solution to
Commercially, NBIS instability is not as problematic as block unintended impurities and damage from the conventional
NBTS and PBTS because it can be readily overcome by adopting plasma-enhanced chemical vapour deposition process; there may

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Articles
be another challenge in obtaining the resistive thin films from the
sputtering target applicable by the d.c. power source. Nevertheless,
we think that there are many candidate materials based on the
following concept: polycrystalline phase for ceramic targets exhib-
its high conductivity but the sputter-deposited amorphous phase
is resistive.
On the other hand, many studies have used a stretched expo-
nential function to analyse the phenomenon of bias instabili-
ties in AOS TFTs9,39–46. This function is often used to explain
the kinetics in disordered systems and expressed as follows:
ΔVth(t) = (Vth(∞) – Vth(0)) × (1 – exp(–t/τ)β), where Vth(∞) is the
threshold voltage when time approaches infinity, Vth(0) is the ini-
tial threshold voltage, τ is a time constant and β is an energy bar-
rier parameter39–46. As shown in Supplementary Fig. 16, we revealed
that the τ and β values significantly change by eliminating the
CO-related impurity: for the stable ITZO TFT, τ = 2.6 × 104 and
β = 0.5; for the unstable ITZO TFT, τ = 2.9 × 103 and β = 0.7. Some
studies in the literature on AOS TFTs have shown that the value of
β does not change44–46. Our understanding is that β changes when
the charge transfer mechanism or origin differs because β is the
parameter reflecting the distribution of the energy barrier. Another
study reported that β considerably differs in a ZnO-based gas sensor
depending on the introduced gas species47. A high-mobility, highly
stable In2O3 TFT has been recently reported, where it was shown
that β differs by the difference in the Fermi levels40. On the other
hand, we confirmed that ΔVth (t → ∞) is different by two orders
of magnitude between the stable and unstable ITZO TFTs. For the
stable ITZO TFT, ΔVth (t → ∞) was only –0.11 V, whereas it was
–16.60 V for the unstable ITZO TFT. This result validates not only
the effect of the CO-related impurity but also the intrinsic potential
of ITZO TFTs for commercial application.
Conclusions
We have reported the origin of the mobility–stability trade-off in
AOS TFTs. The electronic structures and electrical properties of a
range of AOSs were examined. The bilayer-structured TFT revealed
that the NBTS mechanism is mainly attributed to the Fermi-level
shift in the ITZO itself. Higher-mobility AOSs tend to have a
deep ECBM (that is, electron affinity), leading to large differences
in the carrier-doping ability. Shallower donor levels are formed
for higher-mobility AOSs. AOSs with shallow donor levels (small
Ea) should have a relatively small number of donors to obtain the
appropriate carrier density (~1016 cm−3) for TFTs. The variation in
the required donor densities results in great differences in the defect
tolerance. AOSs with a smaller initial donor density suffer more
from externally introduced defects (for example, VO+) or impurities
(for example, H+ or H−). CO-related impurities, which play a role
of gatebias dependent donor, were shown to be the origin of NBTS
instability. Eliminating CO-related impurities, combined with fur-
ther surface passivation, allowed us to fabricate ultrastable ITZO
TFTs with a mobility of 70 cm2 (V s)–1. With such devices, there
may be further unknown impurities introduced during manufac-
turing, which could play additional roles. Nevertheless, our study
has provided an insight and understanding that allows ultrastable
high-mobility AOS TFTs to be fabricated.
Methods
Fabrication of ITZO thin film and characterization. ITZO thin films were
deposited at room temperature via radio-frequency (RF) magnetron sputtering
using 3 in. ceramic targets (In:Sn:Zn = 20:40:40 and 40:40:20 at.%). The following
sputtering parameters were used: RF power, 150 W; target–substrate distance,
110 mm; total pressure, 0.4 Pa; partial oxygen pressure, 25%. The film density
(as shown in Supplementary Fig. 17) and film thickness were measured by
grazing-incidence X-ray reflectivity spectroscopy (SmartLab, Rigaku), and
the crystal structure of the ITZO film was characterized by X-ray diffraction
spectroscopy (SmartLab, Rigaku). The electrical properties of ITZO were
evaluated by a.c.-field Hall effect measurement (ResiTest8400, TOYO) in the
806 Nature Electronics | VOL 4 | November 2021 | 800–807 | www.nature.com/natureelectronics
Nature Electronics
van der Pauw configuration, and the optical bandgap and absorption coefficient
of ITZO were acquired by an ultraviolet–visible spectrometer (UH4150, Hitachi).
Then, 40 nm ITZO films were prepared for thermal desorption spectroscopy
measurement (ESCO) and Auger electron spectroscopy (PHI 710, ULVAC-PHI).
HAXPES was performed at the BL15XU undulator beamline (photon
energyhν =hν 5,953.4hν eV) on 100 nm ITZO films in SPring-8. The energy levels
of conduction band minimum and valence band maximum (ECBM and EVBM) of
the AOSs were determined by using the ultraviolet photoemission spectroscopy,
HAXPES and ultraviolet-visible spectroscopy.
Device fabrication. A schematic of the fabrication method is illustrated in
Supplementary Fig. 5. Bottom-gate and top-contact TFTs were fabricated on
SiO2/p++-silicon substrate. The thickness of the thermally grown SiO2 was
150 nm. The sequential 20 nm ITZO layer was deposited on SiO2 by 150 W RF
magnetron sputtering. After depositing the ITZO layer, the device was subjected
to thermal annealing at 400 °C for 1 h in air. The source/drain electrodes were
constructed by a 5 nm conductive ITZO layer (deposited at 0% partial oxygen
pressure) and a 60 nm gold layer. The channel width and length were patterned
to be 60 and 30 μm (W = 300 µm and L = 50 µm were used only for the devices
shown in Fig. 2 and Supplementary Fig. 1), respectively, by photolithography
(mask aligner MA-10, Mikasa). The lift-off process was employed for all the
patterning procedures. For the NBTS, PBTS and NBIS samples, an additional
ZSO (Zn:Si = 80:20 at.%) layer was deposited on the device by 60 W RF
magnetron sputtering at 25% partial oxygen pressure under 0.4 Pa at a distance
of 80 mm from the target. Thermal annealing (320 °C for 1 h) was performed
again to recover the damage from plasma.
Device characterization. All the devices were measured at a drain–source voltage
of VDS = 0.1 V in a vacuum (1 × 10−3 Pa) by using a B1500A instrument (Keysight).
The NBS conditions were set up at Vth –20 V. NBTS and PBTS were measured
under the following conditions: negative gate bias, Vth –20 V; positive gate bias,
Vth +20 V; temperature, 60 °C. Illumination stress was measured under an LED
light source with the spectrum shown in Supplementary Fig. 14. The spectrum and
illuminance of the LED were detected by a C-7000 SPECTROMASTER instrument
(Sekonic). NBIS was measured under the following conditions: negative gate bias,
Vth –20 V; illuminance, 15,000 lx.
Device simulation. The device characteristics were calculated by a device
simulator (Atlas, Silvaco). The simulation employed a configuration similar to that
of the fabricated device and a mobility model with carrier density dependence48.
The following values were used in this simulation: bandgap, 3.7 eV for ITZO and
4.0 eV for IGO; electron affinity, 4.7 eV for ITZO and 4.5 eV for IGO; mobility of
degenerate states, 40 cm2 (V s)–1 for ITZO and 20 cm2 (V s)–1 for IGO; critical carrier
density, 1 × 1020 cm–3 for ITZO and 4 × 1020 cm–3 for IGO; power factor of mobility,
0.2 for ITZO and 0.5 for IGO.
Electrical parameter extraction and impurity concentration. The
field-effect mobility of the device was calculated by the following equation:
μLinear = WCoxL Vds gmmax , where µLinear is the linear mobility of the device; gmmax is the
maximum transconductance; Cox is the unit area capacitance of the gate dielectric;
Vds is the drain voltage; and W and L are the channel width and length, respectively.
The threshold voltage of the device was estimated when the threshold voltage is at
the value of the following equation: W L × 10 nA. To check the reliability of the device
parameters, the transfer curves of TFTs with different widths and lengths and the
experimentally measured capacitance of SiO2 are shown in Supplementary Fig. 18.
The total amount of CO and CO2 was acquired by multiplying an area factor
by the amount of CO and CO2 contained in the reference powder (CaC2O4). The
area factor was deduced by comparing the integration area under the CO and CO2
peaks between the contaminated ITZO and reference powder (CaC2O4) from the
thermal desorption spectrum.
Data availability
The datasets analysed in this study are available from the corresponding authors
upon reasonable request.
Received: 15 April 2021; Accepted: 13 October 2021;
Published online: 22 November 2021
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Acknowledgements
This work was supported by a grant from the MEXT Element Strategy Initiative:
To Form Core Research Centers (no. JPMXP0112101001).
Author contributions
H.H. and J.K. supervised the project. Y.-S.S., K.S. and Y.S. fabricated and characterized
the samples with support from J.K. M.S. performed the transmission electron microscopy
observations. S.U. performed the HAXPES measurements and analyses. K.A. performed
the device simulation and analyses. Y.-S.S. wrote the manuscript with contributions
mainly from H.H. and J.K. All the authors have given their approval to the final version
of the manuscript.
Competing interests
The authors declare no competing interests.
Additional information
Supplementary information The online version contains supplementary material
available at https://doi.org/10.1038/s41928-021-00671-0.
Correspondence and requests for materials should be addressed to
Junghwan Kim or Hideo Hosono.
Peer review information Nature Electronics thanks Sang-Hee Park and the other,
anonymous, reviewer(s) for their contribution to the peer review of this work.
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